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Metal-Triggered DNA Folding by Different Mechanisms
Wei Deng,Bin Zheng,Wei Ding,Hong Zhu,Hao-jun Liang*
Author NameAffiliationE-mail
Wei Deng Department of Polymer Science and Engineering, University of Science and Technology of China, Hefei 230026, China  
Bin Zheng School of Chemistry and Chemical Engineering, Hefei Normal University, Hefei 230061, China  
Wei Ding Department of Polymer Science and Engineering, University of Science and Technology of China, Hefei 230026, China  
Hong Zhu Department of Polymer Science and Engineering, University of Science and Technology of China, Hefei 230026, China  
Hao-jun Liang* Department of Polymer Science and Engineering, University of Science and Technology of China, Hefei 230026, ChinaCAS Key Laboratory of Soft Matter Chemistry, University of Science and Technology of China, Hefei 230026, China hjliang@ustc.edu.cn 
Abstract:
Metal-mediated base pairs by the interaction between metal ions and artificial bases in oligonucleotides has been widely used in DNA nanotechnology and biosensing technique. Using isothermal titration calorimetry, circular dichroism spectroscopy and fluorescence spectroscopy, the folding process of T-C-rich oligonucleotides (TCO) induced by Hg2+ and Ag+ with the synthetic sequence d(T6C6T6C6T6C6T6) was studied and analyzed. Although thermodynamic data predict that TCO should initially fold into a relatively stable hairpin through two possible pathways of conformational transitions whether Hg2+ or Ag+ were added at first, the mechanisms and final products between the two are entirely different from isothermal titration calorimetry outcomes. When Hg2+ were added first, the haipin was formed through T-Hg-T structure with further stabilization by C-Ag-C after Ag+ addition. However, it is proposed that an unusual metal-base pair for Ag+ binding is generated instead classical C-Ag-C when Ag+ was injected first. Moreover, further confirmation of this unconventional metal-base pair T-Ag-C was verified by circular dichroism and fluorescence spectroscopy.
Key words:  Metal-mediated base pairs, Hg2+ and Ag+, T-C-rich oligonucleotides, Folding mechanisms, T-Ag-C base pair
FundProject:
金属离子诱导下DNA折叠的不同机理
邓伟,郑斌,丁伟,朱红,梁好均*
摘要:
利用等温滴定量热仪、圆二色谱和荧光光谱,研究和分析了人工合成的DNA单链序列d(T6C6T6C6T6C6T6)与Hg2+和Ag+相互作用的折叠过程. 在改变离子添加顺序的情况下,尽管热力学数据显示两种情况下都能通过两种不同反应路径得到一种相对稳定的发夹结构,但等温滴定量热仪数据却显示最终产物形成的机理截然不同.当先加入Hg2+时,发夹结构首先通过T-Hg-T碱基对形成然后C-Ag-C碱基对得到进一步稳定. 然而当先加入Ag+时,通过圆二色谱和荧光分析确认了一种不常见的金属碱基对T-Ag-C取代了经典的C-Ag-C碱基对.
关键词:  金属离子碱基对,Hg和Ag离子,寡聚核苷酸,折叠机理,T-Ag-C碱基对
DOI:10.1063/1674-0068/28/cjcp1503051
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